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Title: Sub‐6 nm Fully Ordered L 1 0 ‐Pt–Ni–Co Nanoparticles Enhance Oxygen Reduction via Co Doping Induced Ferromagnetism Enhancement and Optimized Surface Strain
Abstract

Engineering the crystal structure of Pt–M (M = transition metal) nanoalloys to chemically ordered ones has drawn increasing attention in oxygen reduction reaction (ORR) electrocatalysis due to their high resistance against M etching in acid. Although Pt–Ni alloy nanoparticles (NPs) have demonstrated respectable initial ORR activity in acid, their stability remains a big challenge due to the fast etching of Ni. In this work, sub‐6 nm monodisperse chemically orderedL10‐Pt–Ni–Co NPs are synthesized for the first time by employing a bifunctional core/shell Pt/NiCoOxprecursor, which could provide abundant O‐vacancies for facilitated Pt/Ni/Co atom diffusion and prevent NP sintering during thermal annealing. Further, Co doping is found to remarkably enhance the ferromagnetism (room temperature coercivity reaching 2.1 kOe) and the consequent chemical ordering ofL10‐Pt–Ni NPs. As a result, the best‐performing carbon supportedL10‐PtNi0.8Co0.2catalyst reveals a half‐wave potential (E1/2) of 0.951 V versus reversible hydrogen electrode in 0.1mHClO4with 23‐times enhancement in mass activity over the commercial Pt/C catalyst along with much improved stability. Density functional theory (DFT) calculations suggest that theL10‐PtNi0.8Co0.2core could tune the surface strain of the Pt shell toward optimized Pt–O binding energy and facilitated reaction rate, thereby improving the ORR electrocatalysis.

 
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Award ID(s):
1828019
NSF-PAR ID:
10461196
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Energy Materials
Volume:
9
Issue:
17
ISSN:
1614-6832
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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